1. Highly dispersed nickel site catalysts for diluted CO2 photoreduction to CO with nearly 100% selectivity.
- Author
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Liang, Shujie, Zhong, Xiaohui, Zhong, Zuqi, Deng, Hong, and Wong, Wai-Yeung
- Subjects
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NICKEL catalysts , *PHOTOREDUCTION , *CARBON dioxide , *QUANTUM efficiency , *POLYIMIDES , *POLYMERS , *THERMODYNAMICS - Abstract
Photoconversion of CO 2 into value-added fuels has aroused widespread interest; however, this process is significantly limited by the inefficient thermodynamics and sluggish reaction dynamics in the diluted CO 2. To circumvent these obstacles, we design a bipyridine-based polyimide polymer for anchoring single Ni site for diluted CO 2 photoreduction. The desired Ni single atomic catalysts achieve high generation activity of ∼ 2262 μmol/h with apparent quantum efficiency (A.Q.E.) of 0.20% for CO 2 -to-CO in 0.1 atm CO 2 pressure. No measurable H 2 is produced in the catalytic process, affording nearly 100% CO selectivity over water splitting. This superior activity and selectivity outperform most previous atomical catalysts. Mechanistic analyses elucidate that the highly dispersed Ni atoms act as active sites for effective CO 2 binding and activation, and stabilize the rate-determining step of intermediates for CO generation. This work discloses the relationship between catalytic properties and single atoms for efficient solar-driven diluted CO 2 reduction. [Display omitted] • A novel Bpy-based polyimide polymer was fabricated for anchoring single Ni site. • Single-atom strategy leads to simultaneous increase of activity and selectivity. • Optimized Ni SACs for diluted CO 2 photoreduction to CO with nearly 100% selectivity. • CO 2 binding and activation with regulated intermediate are key for CO 2 reduction. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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